Interface to high-performance periodic coupled-cluster theory calculations with atom-centered, localized basis functions

TL;DR

This paper introduces CC-aims, an interface connecting the FHI-aims quantum chemistry code with the CC4S software, enabling high-performance coupled-cluster calculations for solids using localized atomic orbitals.

Contribution

The paper presents a new interface, CC-aims, that links ab initio codes with the CC4S software, facilitating advanced coupled-cluster calculations for periodic systems.

Findings

Enables high-performance CC calculations for solids

Supports both molecular and periodic systems

Provides a flexible interface for various ab initio codes

Abstract

Coupled cluster (CC) theory is often considered the gold standard of quantum-chemistry. For solids, however, the available software is scarce. We present CC-aims, which can interface ab initio codes with localized atomic orbitals and the CC for solids (CC4S) code by the group of A. Gr\"uneis. CC4S features a continuously growing selection of wave function-based methods including perturbation and CC theory. The CC-aims interface was developed for the FHI-aims code (https://fhi-aims.org) but is implemented such that other codes may use it as a starting point for corresponding interfaces. As CC4S offers treatment of both molecular and periodic systems, the CC-aims interface is a valuable tool, where DFT is either too inaccurate or too unreliable, in theoretical chemistry and materials science alike.